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不同沉淀剂制备CuO-ZnO催化剂甲醛乙炔化反应性能
引用本文:李海涛,郝全爱,王志鹏,班丽君,孟平凡,牛珠珠,高春光,徐亚琳,赵永祥. 不同沉淀剂制备CuO-ZnO催化剂甲醛乙炔化反应性能[J]. 分子催化, 2019, 33(2): 124-131
作者姓名:李海涛  郝全爱  王志鹏  班丽君  孟平凡  牛珠珠  高春光  徐亚琳  赵永祥
作者单位:山西大学 化学化工学院 精细化学品教育部工程研究中心, 山西 太原 030006,山西大学 化学化工学院 精细化学品教育部工程研究中心, 山西 太原 030006,山西大学 化学化工学院 精细化学品教育部工程研究中心, 山西 太原 030006,山西大学 化学化工学院 精细化学品教育部工程研究中心, 山西 太原 030006,山西大学 化学化工学院 精细化学品教育部工程研究中心, 山西 太原 030006,山西大学 化学化工学院 精细化学品教育部工程研究中心, 山西 太原 030006,山西大学 化学化工学院 精细化学品教育部工程研究中心, 山西 太原 030006,山西大学 化学化工学院 精细化学品教育部工程研究中心, 山西 太原 030006,山西大学 化学化工学院 精细化学品教育部工程研究中心, 山西 太原 030006
基金项目:国家自然科学基金(U1710221,21503124);山西省国际合作项目(201603D421025,201703D421034)
摘    要:分别以NaOH、Na2CO3、NaHCO3为沉淀剂,采用共沉淀法制备了Cu:Zn摩尔比为2:1的CuO-ZnO催化剂,利用氢气程序升温还原(H2-TPR)、热重(TG)、X射线衍射(XRD)及拉曼光谱(Raman)等技术对催化剂进行了表征,结合甲醛乙炔化活性评价,研究了沉淀剂对催化剂结构及催化性能的影响.结果表明,不同沉淀剂对催化剂中活性组分分散度有较大影响,进而在甲醛乙炔化合成1,4-丁炔二醇反应中表现出不同的催化活性.以Na2CO3为沉淀剂制备的催化剂中形成CuO-ZnO固溶体,提高了CuO的分散度及Cu+在还原性气氛下的稳定性,经活化后可生成较多的活性物种炔化亚铜,表现出最佳的炔化反应活性与1,4-丁炔二醇选择性.

关 键 词:CuO-ZnO  甲醛乙炔化  1,4-丁炔二醇  沉淀剂
收稿时间:2019-01-16
修稿时间:2019-02-19

Study on Catalytic Performance of CuO-ZnO Catalyst Prepared by Different Precipitants
LI Hai-tao,HAO Quan-ai,WANG Zhi-peng,BAN Li-jun,MENG Ping-fan,NIU Zhu-zhu,GAO Chun-guang,XU Ya-lin and ZHAO Yong-xiang. Study on Catalytic Performance of CuO-ZnO Catalyst Prepared by Different Precipitants[J]. Journal of Molecular Catalysis (China), 2019, 33(2): 124-131
Authors:LI Hai-tao  HAO Quan-ai  WANG Zhi-peng  BAN Li-jun  MENG Ping-fan  NIU Zhu-zhu  GAO Chun-guang  XU Ya-lin  ZHAO Yong-xiang
Affiliation:Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemisry and Chemical Engineering, Shanxi University, Taiyuan 030006, China,Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemisry and Chemical Engineering, Shanxi University, Taiyuan 030006, China,Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemisry and Chemical Engineering, Shanxi University, Taiyuan 030006, China,Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemisry and Chemical Engineering, Shanxi University, Taiyuan 030006, China,Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemisry and Chemical Engineering, Shanxi University, Taiyuan 030006, China,Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemisry and Chemical Engineering, Shanxi University, Taiyuan 030006, China,Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemisry and Chemical Engineering, Shanxi University, Taiyuan 030006, China,Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemisry and Chemical Engineering, Shanxi University, Taiyuan 030006, China and Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemisry and Chemical Engineering, Shanxi University, Taiyuan 030006, China
Abstract:CuO-ZnO catalyst with Cu:Zn molar ratio of 2:1 was prepared by coprecipitation method using NaOH, Na2CO3 and NaHCO3 as precipitants. The catalysts were characterized by thermogravimetry (TG), hydrogen-programmed reduction (H2-TPR), X-ray diffraction (XRD) and Raman spectroscopy (Raman). Combined with the evaluation of formaldehyde acetylation activity, the effect of precipitation agent on the structure and cataly-tic performance of the catalyst were studied. The results show that different precipitants have a great influence on the dispersion of active components in the catalyst, and then show different catalytic activities in the reaction of formaldehyde acetylation to 1,4-butynediol. In the CZ(Na2CO3) catalyst, the active species CuO and ZnO form a CuO-ZnO solid solution, which improves the dispersion of CuO and the stability of Cu+ under reducing atmosphere. After activation, more active central species acetylene cuprous can be formed. The optimum alkyneization activity is selective with 1,4-butynediol.
Keywords:CuO-ZnO  formaldehyde acetylation  1,4-butynediol  precipitants
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